Hydrogen degradation of structural materials, such as nickel-based alloys, is characterized by both enhanced dislocation processes and grain boundary decohesion leading to intergranular fracture. Nanoindentation and scanning probe microscopy (SPM) were used to characterize slip transfer across high- and low-energy grain boundaries in commercially pure nickel before and after hydrogen charging. Both high-energy random boundaries and low-energy recrystallization twins were identified for indentation using electron backscatter diffraction. Nanoindentation produced local deformation along grain boundaries, causing material pile-up and slip steps; thermal hydrogen-charging altered the observed response to local deformation. Additional indentation within specific grains indicated hydrogen charging reduces modulus. Coupled nanoindentation and SPM investigations provide a unique method for analyzing local hydrogen effects as a function of grain boundary type, which can be used to develop grain boundary engineered materials. Partial support provided by Sandia National Laboratories, a Lockheed Martin Company for USDOE NNSA under contract DE-AC04-94AL85000.